The fibers based on thermoplastic partially crystalline polyetherimide R-BAPB modified by vapor grown carbon nanofibers (VGCF) were prepared by melt extrusion, exposed to orientational drawing, and crystallized. All of the samples were examined by scanning electron microscopy, X-ray scattering, and differential scanning calorimetry to study how the carbon nanofiller influences on the internal structure and crystallization behavior of the obtained R-BAPB fibers. The mechanical properties of the composite R-BAPB fibers were also determined. It was found that VGCF nanoparticles introduced into R-BAPB polyimide can act as a nucleating agent that leads, in turn, to significant changes in the composite fibers morphology as well as thermal and mechanical characteristics. VGCF are able to improve an orientation degree of the R-BAPB macromolecules along the fiber direction, accelerate crystallization rate of the polymer, and enhance the fiber stability during crystallization process.

Samples of composite materials based on high-performance semicrystalline polyimide R-BAPB (based on the dianhydride R: 1,3-bis-(3′,4,-dicarboxyphenoxy)benzene and diamine BAPB: 4,4′-bis-(4″-aminophenoxy)diphenyl)) filled with carbon nanofibers and micron-sized discrete carbon fibers were obtained by FFF printing for the first time. The viscosity of melts of the composites based on R-BAPB, thermal, mechanical characteristics of the obtained composite samples, their internal structure, and biocompatibility were studied. Simultaneously with FFF printing, samples were obtained by injection molding. The optimal concentrations of carbon fillers in polyimide R-BAPB for their further use in FFF printing were determined. The effect of the incorporation of carbon fillers on the porosity of the printed samples was investigated. It was shown that the incorporation of carbon nanofibers reduces the porosity of the printed samples, which leads to an increase in deformation at break. Modification of polyimide with discrete carbon fibers increases the strength and Young’s modulus sufficiently but decreases the deformation at break. The cytotoxicity analysis showed that the obtained composite materials are bioinert.

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In the process of this work, an oligoimide FT-BAPB-R-BAPB-FT was synthesized, the particles of which consist of numerous lamellas having a semi-crystalline structure. On the DSC thermogram of oligoimide powder, two endo peaks were observed at 281.1°C and 306.4°C. A unique WAXS experiment was performed in-situ by heating the reactor oligoimid powder in a heat chamber. There was no significant difference in the X-ray profiles when the sample was heated. It should be noted that the transformation of the crystalline cell does not occur until the sample melts. It was revealed that the degree of crystallinity decreases during heating. We believe that the low-temperature endopeak is associated with the melting of small crystallites and amorphization of the sample. However, a significant increase in crystal size was found to be a result of recrystallization. Thus, the high-temperature endopic corresponds to the melting of larger crystallites.

HDPE-based composite fibers filled by original and annealed carbon nanodiscs (oND and aND, respectively) were prepared by melt extrusion technology with high-temperature orientational drawing up to draw ratio DR = 8. The thermal properties of the obtained fibers were investigated by DSC and TGA methods. It was shown that the nanofillers can be influenced by high temperatures, at which the molecular mobility in the interlamellar regions became active, while the melting point and the crystallinity degree of the samples were not affected. Short- and long-term mechanical properties of the nanocomposite fibers were studied as well. Very rare mechanical testing of the knotted fibers was carried out and, as a result, a decrease of the knot strength up to 35% was detected. It was also revealed that the carbon nanodiscs do not reinforce the composite fibers and play a negative role in the creep processes, while the Young’s modulus can be improved by 2 times for the oriented samples.